Tracking the FeIV(O) intermediate and O–O bond formation of a nonheme iron catalyst for water oxidation

2017 ◽  
Vol 53 (65) ◽  
pp. 9063-9066 ◽  
Author(s):  
Bing Yang ◽  
Qing-Qing Yang ◽  
Xin Jiang ◽  
Bin Chen ◽  
Chen-Ho Tung ◽  
...  
Keyword(s):  
Oxygen Evolution ◽  
Water Oxidation ◽  
Iron Catalyst ◽  
Bond Formation ◽  
Nonheme Iron ◽  
High Valent

We describe here a new complex 1 by subtle modulation of the TPA ligand and succeed in capturing the high-valent FeIV(O) species, which is responsible for the O–O bond formation and oxygen evolution with higher efficiency.

scholarly journals Formation of CoIV=O intermediate at the Boundary of the “Oxo-wall” Induces Water Oxidation

2020 ◽  
Author(s):  
Roman Ezhov ◽  
Alireza Ravari ◽  
Gabriel Bury ◽  
Paul Smith ◽  
Yulia Pushkar
Keyword(s):  
Hydrogen Bonding ◽  
Water Splitting ◽  
Oxygen Evolution ◽  
Water Oxidation ◽  
Artificial Photosynthesis ◽  
Bond Formation ◽  
Nucleophilic Attack ◽  
Earth Abundant ◽  
3D Elements

Abstract Development of economically viable artificial photosynthesis requires use of 3d metal-based catalysts. Water oxidation by [Co4O4]n+ cubane mimics water splitting by CaMn4O5 cluster in Nature but the exact mechanism of O-O bond formation is presently unknown. We demonstrate first in situ detection CoIV=O (~ 1.67 Å) moiety formed upon activation of [Co4O4Py4Ac4]0 (Py = pyridine and Ac = CH3COO−) towards O-O bond formation. Combined spectroscopic and DFT analyses show that the intermediate active in O-O bond formation has two CoIV centers and at least one CoIV=O unit of strong radicaloid character that participates in O-O bond formation via water nucleophilic attack. The multimetallic structure of the cubane provides unique stabilization for CoIV=O + H2O = Co-OOH + H+ transition with the carboxyl accepting the proton and the bridging oxygen stabilizing the peroxide via hydrogen bonding. Results are important for development of oxygen evolution catalysts based on Earth-abundant 3d elements.

scholarly journals Synthetic control and empirical prediction of redox potentials for Co4O4 cubanes over a 1.4 V range: implications for catalyst design and evaluation of high-valent intermediates in water oxidation

2017 ◽  
Vol 8 (6) ◽  
pp. 4274-4284 ◽  
Author(s):  
Andy I. Nguyen ◽  
Jianing Wang ◽  
Daniel S. Levine ◽  
Micah S. Ziegler ◽  
T. Don Tilley
Keyword(s):  
Cobalt Oxide ◽  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Water Oxidation ◽  
Catalyst Design ◽  
Synthetic Control ◽  
Redox Potentials ◽  
Empirical Prediction ◽  
High Valent

The oxo-cobalt cubane unit [Co4O4] is of interest as a homogeneous oxygen-evolution reaction (OER) catalyst, and as a functional mimic of heterogeneous cobalt oxide OER catalysts.

Controllable growth of graphdiyne layered nanosheets for high-performance water oxidation

2021 ◽  
Author(s):  
Shuya Zhao ◽  
Yurui Xue ◽  
Zhongqiang Wang ◽  
Zhiqiang Zheng ◽  
Xiaoyu Luan ◽  
...  
Keyword(s):  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Water Oxidation ◽  
High Performance ◽  
Low Cost ◽  
Highly Active ◽  
Controllable Growth

Developing highly active, stable and low-cost electrocatalysts capable of an efficient oxygen evolution reaction (OER) is urgent and challenging.

Bifunctional citrate-Ni0.9Co0.1(OH)x layer coated fluorine-doped hematite for simultaneous hole extraction and injection towards efficient photoelectrochemical water oxidation

Nanoscale ◽  
2021 ◽  
Author(s):  
Peng Wang ◽  
Feng Li ◽  
Xuefeng Long ◽  
Tong Wang ◽  
Huan Chai ◽  
...  
Keyword(s):  
Surface Modification ◽  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Water Oxidation ◽  
Surface Oxygen ◽  
Co Catalyst ◽  
Photoelectrochemical Water Oxidation

Surface modification by loading a water oxidation co-catalyst (WOC) is generally considered to be an efficient means to optimize the sluggish surface oxygen evolution reaction (OER) of hematite photoanode for...

High-valent Zirconium-doping modified Co3O4 weave-like nanoarray boosts oxygen evolution reaction

2021 ◽  
pp. 161172
Author(s):  
Guijin Yang ◽  
Botao Zhu ◽  
Yujun Fu ◽  
Jing Zhao ◽  
Yanna Lin ◽  
...  
Keyword(s):  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Zirconium Doping ◽  
High Valent

Rutile TiO2 single crystals delivering enhanced photocatalytic oxygen evolution performance

Nanoscale ◽  
2021 ◽  
Author(s):  
Bing Fu ◽  
Zhijiao Wu ◽  
Kai Guo ◽  
Lingyu Piao
Keyword(s):  
Catalytic Activity ◽  
Single Crystals ◽  
Oxygen Evolution ◽  
Water Oxidation ◽  
Charge Separation ◽  
High Surface ◽  
Rutile Tio2 ◽  
Highly Efficient ◽  
Photogenerated Charge Separation

Owing to their scientific and technological importance, the development of highly efficient photocatalytic water oxidation systems with rapid photogenerated charge separation and high surface catalytic activity has highly desirable for...

Oriental and robust anchoring of Fe via anodic interfacial coordination assembly on ultrathin Co hydroxides for efficient water oxidation

Nanoscale ◽  
2021 ◽  
Author(s):  
Ya-Nan Zhou ◽  
Ruo-Yao Fan ◽  
Yu-Ning Cao ◽  
Hui-Ying Wang ◽  
Bin Dong ◽  
...  
Keyword(s):  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Water Oxidation ◽  
Active Sites

The oriental distribution and strong conjunction of Fe active sites in multiple metals hydroxides are very crucial to modulate the activity and stability for efficient oxygen evolution reaction (OER). Whereas,...

Soluble lanthanide-transition-metal clusters Ln36Co12 as effective molecular electrocatalysts for water oxidation

2021 ◽  
Vol 57 (29) ◽  
pp. 3611-3614
Author(s):  
Rong Chen ◽  
Chao-Long Chen ◽  
Ming-Hao Du ◽  
Xing Wang ◽  
Cheng Wang ◽  
...  
Keyword(s):  
Transition Metal ◽  
Transition Metals ◽  
Synergistic Effect ◽  
Water Oxidation ◽  
Metal Clusters ◽  
Bond Formation ◽  
Transition Metal Clusters ◽  
Oxidation Activity ◽  
Acidic Conditions ◽  
Effective Water

The stable 48-metal Ln36Co12 clusters show an effective water oxidation activity under weak acidic conditions because of the synergistic effect between lanthanide and transition metals in O–O bond formation.

Reaction Mechanism of a Nonheme Iron Enzyme Catalyzed Oxidative Cyclization via C–C Bond Formation

2018 ◽  
Vol 21 (1) ◽  
pp. 228-232 ◽  
Author(s):  
Wei-chen Chang ◽  
Zhi-Jie Yang ◽  
Yueh-Hua Tu ◽  
Tun-Cheng Chien
Keyword(s):  
Reaction Mechanism ◽  
Bond Formation ◽  
Oxidative Cyclization ◽  
Nonheme Iron
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